Ultra-narrow room-temperature emission from single CsPbBr3 perovskite quantum dots

Gabriele Rainò (), Nuri Yazdani, Simon C. Boehme, Manuel Kober-Czerny, Chenglian Zhu, Franziska Krieg, Marta D. Rossell, Rolf Erni, Vanessa Wood, Ivan Infante and Maksym V. Kovalenko ()
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Gabriele Rainò: ETH Zurich
Nuri Yazdani: ETH Zurich
Simon C. Boehme: ETH Zurich
Manuel Kober-Czerny: ETH Zurich
Chenglian Zhu: ETH Zurich
Franziska Krieg: ETH Zurich
Marta D. Rossell: Empa–Swiss Federal Laboratories for Materials Science and Technology
Rolf Erni: Empa–Swiss Federal Laboratories for Materials Science and Technology
Vanessa Wood: ETH Zurich
Ivan Infante: Vrije Universiteit Amsterdam
Maksym V. Kovalenko: ETH Zurich

Nature Communications, 2022, vol. 13, issue 1, 1-8

Abstract: Abstract Semiconductor quantum dots have long been considered artificial atoms, but despite the overarching analogies in the strong energy-level quantization and the single-photon emission capability, their emission spectrum is far broader than typical atomic emission lines. Here, by using ab-initio molecular dynamics for simulating exciton-surface-phonon interactions in structurally dynamic CsPbBr3 quantum dots, followed by single quantum dot optical spectroscopy, we demonstrate that emission line-broadening in these quantum dots is primarily governed by the coupling of excitons to low-energy surface phonons. Mild adjustments of the surface chemical composition allow for attaining much smaller emission linewidths of 35−65 meV (vs. initial values of 70–120 meV), which are on par with the best values known for structurally rigid, colloidal II-VI quantum dots (20−60 meV). Ultra-narrow emission at room-temperature is desired for conventional light-emitting devices and paramount for emerging quantum light sources.

Date: 2022
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DOI: 10.1038/s41467-022-30016-0

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